CN105957983A - Electrochemical devices for use in extreme conditions - Google Patents

Electrochemical devices for use in extreme conditions Download PDF

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Publication number
CN105957983A
CN105957983A CN201610506323.7A CN201610506323A CN105957983A CN 105957983 A CN105957983 A CN 105957983A CN 201610506323 A CN201610506323 A CN 201610506323A CN 105957983 A CN105957983 A CN 105957983A
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Prior art keywords
ionic liquid
negative electrode
battery
temperature
alloy
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CN201610506323.7A
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Chinese (zh)
Inventor
W·张
C·巴瑟
R·费雷克
I·库珀
A·蒂鲁瓦纳玛莱
J·H-F·程
J·R·王
S·琼斯
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Prad Research and Development Ltd
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Prad Research and Development Ltd
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Publication of CN105957983A publication Critical patent/CN105957983A/en
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/14—Cells with non-aqueous electrolyte
    • H01M6/16—Cells with non-aqueous electrolyte with organic electrolyte
    • H01M6/162—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte
    • H01M6/164—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte by the solvent
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/22—Electrodes
    • H01G11/30—Electrodes characterised by their material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/22—Electrodes
    • H01G11/30—Electrodes characterised by their material
    • H01G11/32—Carbon-based
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/22—Electrodes
    • H01G11/30—Electrodes characterised by their material
    • H01G11/46—Metal oxides
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/52—Separators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
    • H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
    • H01G9/004—Details
    • H01G9/04—Electrodes or formation of dielectric layers thereon
    • H01G9/06—Mounting in containers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/381—Alkaline or alkaline earth metals elements
    • H01M4/382—Lithium
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/40—Alloys based on alkali metals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H01M4/5835—Comprising fluorine or fluoride salts
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/669—Steels
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/72—Grids
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/72—Grids
    • H01M4/74—Meshes or woven material; Expanded metal
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings, jackets or wrappings of a single cell or a single battery
    • H01M50/116—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material
    • H01M50/117—Inorganic material
    • H01M50/119—Metals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings, jackets or wrappings of a single cell or a single battery
    • H01M50/14—Primary casings, jackets or wrappings of a single cell or a single battery for protecting against damage caused by external factors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/14—Cells with non-aqueous electrolyte
    • H01M6/16—Cells with non-aqueous electrolyte with organic electrolyte
    • H01M6/162—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte
    • H01M6/166—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte by the solute
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H01M2300/0028—Organic electrolyte characterised by the solvent
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H01M2300/0045—Room temperature molten salts comprising at least one organic ion
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/40—Alloys based on alkali metals
    • H01M4/405—Alloys based on lithium
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/13—Energy storage using capacitors

Abstract

An electrochemical device, such as a battery or power source, provides improved performance under stringent or extreme conditions. Such an electrochemical device for use in high temperature conditions may include at least a cathode, a lithium-based anode, a separator, and an ionic liquid electrolyte. This device also may include a current collector and housing that are electrochemically inert with respect to other components of the device. This electrochemical device may operate at temperatures ranging from 0 to 180, 200, 220, 240, and 260 DEG C.

Description

The electrochemical appliance under extreme conditions used
The application is Application No. 201180018139.3, filing date in April, 2011 6 days, the patent application of entitled " electrochemical appliance under extreme conditions used " Divisional application.
Related application
Subject application requires filed in 6 days April in 2010 according to 35U.S.C. § 199 (e), Entitled " Power Sources and Methods of Providing Power to a Device " The right of U.S. Provisional Application case the 61/321st, 309, described application case is in full to draw Mode be incorporated herein.
Technical field
Present disclosure is broadly directed to change into chemical energy the electrochemistry of electrochemical source of current Device, and relate more specifically to the electrochemical appliance that can under extreme conditions use.
Background of invention
The increase of energy demand and be easier to the declining of oilfield reserve of exploitation in global range Exhaust promotion and to the more severe or exploration of extreme environment (such as deep water) and carry out underground heat Can probing.These adverse circumstances are usually directed to high pressure and/or hot conditions.These high pressure And/or hot conditions generally proposes more harsh wanting to the device powered to underground equipment Ask.Past, lithium-thionyl chloride (LiSOCl2) battery as oil well exploit In widely used power supply.But, LiSOCl2Battery itself is due to the low fusing temperature of lithium Degree and at high temperature unstable and these physical propertys are prone to LiSOCl2The operation of battery Temperature limiting is the highest 200 DEG C.LiSOCl2Battery exceedes these limit values may cause electricity Pond fault, performance degradation and potential battery explosion.
Brief summary of the invention
The embodiment of present disclosure substantially provides a kind of electricity under hot conditions Chemical devices, described device includes at least one negative electrode, lithio anode, ionic liquid electricity Solve matter and barrier film, wherein said device from about 0 DEG C to 180 DEG C, 200 DEG C, 220 DEG C, Run at a temperature of in the range of 240 DEG C or 260 DEG C.Negative electrode can be to have chemical formula CFxPerfluorocarbon, wherein x is in the scope of 0.3 to 1.Perfluorocarbon can be without surface Formed in the case of activating agent.Or, negative electrode can include MnO2Or FeS2.Lithio sun Pole is selected from including lithium, having chemical formula LixMyBianry alloy and Li-B-Mg or The group of the ingot alloy of Li-Mg-xM, wherein M be magnesium, silicon, aluminum, stannum, boron, calcium or A combination thereof.Ionic liquid electrolyte can by selected from include EMI, MPP, BMP, In the ionic liquid of the group of BTMA, DEMMoEA, hydridization electrolyte and its mixture Dissolve lithium salts and formed.Barrier film is selected from from including fibrous glass, PTFE, polyamides At least one material of imines, aluminium oxide, silicon dioxide and zirconic group.
This electrochemical appliance that embodiment according to present disclosure is formed can include By at least one collector body formed of llowing group of materials: nickel, titanium, rustless steel, aluminum, silver, Gold, platinum, carbon cloth and carbon cladding titanium or rustless steel.Negative electrode also can be forced into foam or grid On to form collector body.This electrochemical appliance may also include by least the one of llowing group of materials Kind formed shell: rustless steel, high nickel and stainless steel, titanium, precious metal electroplating rustless steel and Nonmetal-coated rustless steel.Or, negative electrode can be attached directly to the shell of device.Dress Put and can have selected from including bobbin structure, thin layer coating, spiral winding structure and medium bed The structure of the group of package structure.
Another embodiment of present disclosure relates to high temperature power supply, and it includes perfluorocarbon Negative electrode, lithio anode, barrier film and ionic liquid electrolyte, wherein power supply is from about 0 DEG C Run at a temperature of in the range of 260 DEG C.Ionic liquid electrolyte can be by being selected from Including EMI, MPP, BMP, BTMA, DEMMoEA, hydridization electrolyte and its The ionic liquid of the group of mixture dissolves lithium salts and is formed.Lithio anode is selected from including Lithium, there is chemical formula LixMyBianry alloy and the ingot of Li-B-Mg and Li-Mg-xM The group of alloy, wherein M is magnesium, silicon, aluminum, stannum, boron, calcium or a combination thereof.
Another embodiment of present disclosure relates to the battery under hot conditions, Described battery includes that perfluorocarbon negative electrode, corresponding weight ratio are the Li-B-Mg of 64:32:4 at a low price Anode and ionic liquid electrolyte, wherein battery is from the scope of about 0 DEG C to 260 DEG C Run at a temperature of Nei.Perfluorocarbon can have chemical formula CFx at a low price, and wherein x has The value of 0.9.Ionic liquid electrolyte can be in the concentration of the LiTFSI in being dissolved in MPP In the range of 0.1M to 1M.Battery may also include barrier film, and described barrier film includes choosing From including polyimides, PTFE, porous ceramics, such as aluminium oxide, silicon dioxide or oxygen Change the materials at two layers of the group of zirconium or fibrous glass and a combination thereof.Described battery may also include by Nickel, rustless steel, aluminum, silver, gold, titanium, carbon cloth or carbon cladding rustless steel or titanium are formed Netted collector body.
The application also includes following items:
1. the electrochemical appliance under hot conditions, described device includes:
Negative electrode, lithio anode, ionic liquid electrolyte and barrier film,
Wherein said device runs at a temperature of in the range of 0 DEG C to 180 DEG C.
2., according to the device described in project 1, wherein said negative electrode is selected from including following thing The group of matter:
There is the perfluorocarbon of chemical formula CFx, wherein x in the scope of 0.3 to 1, MnO2 and FeS2.
3. according to the device according to any one of prior projects, described device also include by Llowing group of materials at least one formed collector body: nickel, titanium, rustless steel, aluminum, silver, Gold, platinum, carbon cloth, carbon cladding titanium and carbon cladding rustless steel.
4., according to the device according to any one of prior projects, wherein said negative electrode is pressed To form collector body on foam or grid.
5., according to the device according to any one of prior projects, described device also includes:
By at least one shell formed of llowing group of materials: rustless steel, high nickel and stainless steel, Titanium, precious metal electroplating rustless steel and nonmetal-coated rustless steel.
6., according to the device according to any one of prior projects, wherein said negative electrode is direct It is attached to described shell.
7. according to the device according to any one of prior projects, wherein said lithio anode Group selected from including following material:
Lithium, there is the bianry alloy of chemical formula LixMy, there is chemical formula Li1-xMx Bianry alloy and the ingot alloy of Li-B-Mg or Li-Mg-xM, wherein M be magnesium, Silicon, aluminum, stannum, boron, calcium, zinc and a combination thereof.
8. according to the device according to any one of prior projects, wherein said ionic liquid Electrolyte is by dissolving lithium salts in the ionic liquid of group including following material Formed:
EMI, MPP, BMP, BTMA, DEMMoEA, hydridization electrolyte and its Mixture.
9., according to the device according to any one of prior projects, described device has and is selected from Structure including the group of having structure:
Bobbin structure, thin layer coating, spiral winding structure and medium bed package structure.
10., according to the device according to any one of prior projects, wherein said barrier film is selected from At least one material from the group including llowing group of materials:
Fibrous glass, PTFE, polyimides, aluminium oxide, silicon dioxide and zirconium oxide.
11. according to the device described in project 1, and wherein said device is from 0 DEG C to 200 DEG C Run at a temperature of in the range of.
12. according to the device described in project 1, and wherein said device is from 0 DEG C to 220 DEG C Run at a temperature of in the range of.
13. according to the device described in project 1, and wherein said device is from 0 DEG C to 240 DEG C Run at a temperature of in the range of.
14. according to the device described in project 1, and wherein said device is from 0 DEG C to 260 DEG C Run at a temperature of in the range of.
Accompanying drawing is sketched
In order to present disclosure and its feature are more fully understood, now combine drawings below With reference to being described below, wherein:
Fig. 1 describes to contact carbon according to the embodiment of present disclosure in high temperature exposure CF after cladding titaniumxThe x-ray diffraction analysis of cathode material；
Fig. 2 describes contacting not in high temperature exposure of the embodiment according to present disclosure CF after rust steel 316xThe x-ray diffraction analysis of cathode material；
Fig. 3 describes to contact nickel according to the embodiment of present disclosure in high temperature exposure CF after alloy 625xThe x-ray diffraction analysis of cathode material；
Fig. 4 describes the differential scanning amount of the anode of the embodiment according to present disclosure Heat (DSC) is analyzed；
Fig. 5 describes the ionic liquid electrolyte of the embodiment according to present disclosure Thermogravimetric analysis (TGA) curve；
Fig. 6 describes the different ionic liquid electrolysis of the embodiment according to present disclosure The dsc analysis of matter；
Fig. 7 describes the different ionic liquid electrolysis of the embodiment according to present disclosure The CF of matterxThe dsc analysis of negative electrode/electrolyte half-cell structure；
Fig. 8 describes the different ionic liquid electrolysis of the embodiment according to present disclosure The dsc analysis of the lithio anode/electrolyte half cell configuration of matter；
Fig. 9 describes putting of the high-temperature battery of the embodiment formation according to present disclosure Electricity curve；
The voltage that Figure 10 describes the high-temperature battery of the embodiment according to present disclosure is bent Line.
Detailed description of the invention
Functional cells chemistry is based on having certain electric kinetic potential (emf) to drive in the battery The electrochemical couple of streaming current flowing.Battery relates at least one electrochemical reaction, its During electric discharge, the interface between spaning electrode electrolyte together occurs.Therefore, electrochemistry The assembly of device must be compatible with each other.For hot conditions, as may be at oil field underground mining With the hot conditions occurred in production operation, device assembly also should be exposed to extreme condition Time thermally-stabilised.Other assembly of electrochemical appliance, as battery case and collector body also need by Structure bears these extreme conditions.
The embodiment of present disclosure provides electrochemical appliance, such as battery or power supply, its Chemical energy is changed into electrochemical source of current, and can provide under harsh or extreme condition and change The performance entered.Described device comprises the steps that at least one negative electrode, i.e. includes perfluorocarbon at a low price Or the anelectrode of carbon monofluoride；Anode, i.e. negative electrode；And ionic liquid electrolyte.Institute State device may also include collector body and include that other assembly for device is electrochemically The shell of inert material.Described device also should include barrier film, and described barrier film can be physically With two electrodes of electric isolution, allow the flowing of ion current spaning electrode simultaneously.
Different device assembly-anode, negative electrode, electrolyte, collector body, barrier film and electricity Pond shell can be formed by the material of the reliable energy supply allowed across wide temperature range of operation. More specifically, form the material of the electrochemical appliance of the embodiment according to present disclosure Being configurable under 200 DEG C or higher temperature run, described temperature is about lithium-thionyl The current operational limit of acyl chlorides (LTC) battery.
Return to the negative electrode of the electrochemical appliance that the embodiment according to present disclosure is formed Assembly, solid state cathode, as low price perfluorocarbon or carbon monofluoride can be used for extreme high temperature bar Part.The cathode material of these types can about 350 DEG C to 600 DEG C at a temperature of synthesize. Like this, it is chemically stable and will not thermally decompose in the range of higher temperature.
Perfluorocarbon is to have general. formula CF at a low pricex, wherein the scope of x is from about 0.3 Carbon to 1-fluorine intercalation compound.Fluorination number in the range of this can ensure that the good of negative electrode Good electric conductivity and increase the power density of cathode material.Higher fluorination in the range of this Number, as 0.9 or more High Availabitity in supporting the application of high power capacity/low rate.But this scope Interior more less fluorinated number can be used for obtaining high working voltage, when electric discharge starts without electricity Calendering is late.
Perfluorocarbon cathode material can use the array of feasible precursor material to make, including but It is not necessarily limited to activated carbon, nano-sized carbon and graphite.Precursor material could generally have small particles Size is to provide bigger surface area and to allow material to fill into more high density structure.This Individual larger surface area and more high density structure may additionally facilitate more power and higher energy makes With.
Additionally, the negative electrode according to the embodiment of present disclosure generally can be without except solvent Formed in the case of component in addition, such as water and/or isopropanol, binding agent and Super P (carbon).This is departing from the conventional cathode side of being formed using the additive such as surfactant Method.In the embodiment of present disclosure, negative electrode is formed as CFx/ carbon/binding agent, Corresponding weight ratio is 85/10/5.
Further, it should be appreciated that the material in addition to carbon monofluoride and low price perfluorocarbon can be used as root Cathode assembly according to the electrochemical appliance that the embodiment of present disclosure is formed.Substitute Cathode material can include MnO2And FeS2And a combination thereof.MnO2Based on dsc analysis Assessment and about 100 DEG C to 150 DEG C within the temperature range of functional.FeS2Also Represent and MnO2Similar character and performance.
Collector body can be used for improving the negative electrode of the embodiment according to present disclosure and utilizes Rate.Such as, selected cathode material can be forced into by including but not limited to nickel, Titanium, aluminum, noble metal, such as silver, gold or platinum, carbon cloth, rustless steel and carbon cladding rustless steel Material formed metal foam or grid on.
Foam can give the larger surface area about cathode material and contact.This bigger table Area can improve cathode material to the degree of adhesion of substrate and through the fax of cathode material Lead.Although grid is likely to be of the less surface contact of relevant cathode material compared with foam Area, but it stills provide the rate capacity similar with foam and similar capacity.Non- The use of metal current collector and/or include on the current collector carbon coating can improve rotproofness with Avoid causing in use the potential etching problem of device short circuit.
Use the effectiveness of the different collector body of X-ray diffraction cathode analysis assessment.Negative electrode Sample maintains to contact with different current collector material at 220 DEG C and reaches 150 hours and make subsequently Use X-ray diffraction analysis negative electrode.Fig. 1 to Fig. 3 depicts high temperature exposure contact respectively CF after carbon cladding titanium, Stainless steel 316 and nickel alloy 625xThe x-ray of cathode material Diffraction analysis.These results are depicted as intensity (a.u.) to Cu K α 2 θ (spending).This It is permissible that a little x-ray diffraction results disclose carbon cladding titanium, Stainless steel 316 and nickel alloy 625 It it is effective collector body.These materials are the most stable for the corrosion under test condition, because of For not finding corrosion by-products and CFxContent keeps identical.However, it should be understood that other material Material, including but not limited to aluminum, nickel, titanium, silver, gold, platinum, rustless steel, carbon cloth Collector body is can be used as without deviating from present disclosure with rustless steel or the titanium of carbon coated.
But, in some embodiments of present disclosure, cathode material can be the most attached It is connected to crust of the device to remove the needs to colelctor electrode from.This direct attachment can also be dispersed The reaction heat that may produce during discharging.
Return to the anode assemblies of the device that the embodiment according to present disclosure is formed, mistake Going, pure lithium is often used as LiSOCl2The anode of battery.But, because pure lithium has greatly The fusion temperature of about 180 DEG C, so being incorporated to the embodiment party according to present disclosure by pure lithium The device that case is formed may make the maximum temperature that plant running is limited to about 175 DEG C. Although can be at up to 175 DEG C as the embodiment of the present disclosure of anode including pure lithium Under properly functioning, but this may cause such a device when being exposed to extreme condition Bad performance.
The anode of the embodiment according to present disclosure may be included in be had under higher temperature There is the material of high thermal stability, but described material may reduce such a electrochemistry The emf of system.In some embodiments, lithium can form alloy with the second element, as Calcium, aluminum, zinc and magnesium.These lithium-base alloy materials can be steady at a temperature of about 260 DEG C Fixed.These lithium alloys can discharge lithium ion during discharging but the most at high temperature physics melts Change.
Pure lithium or different lithium alloy can be used for the embodiment according to present disclosure and formed Device in.Alloy can include non-solution binary lithium alloy, and the purest lithium can be included in knot Structure matrix L i(x)M(y)Or Li1-xMxIn, and M can represent magnesium, silicon, aluminum, stannum, boron, Calcium, zinc or a combination thereof.Such as, lithium magnesium can be used as the lithium bianry alloy of higher temperature battery. Second constituent content of these alloys can be depending on required temperature upper limit and relevant putting Electric loading curve and change to 25% weight ratio from 1% weight ratio.But in order to by anode Fusion temperature bring up to much higher value (such as about 210 DEG C or bigger temperature), Ke Nengxu More substantial magnesium is incorporated in alloy.These more substantial magnesium alloy may be caused harder and And crisp and therefore may make anode preparation more complicated and make battery assembling and make more tired Difficult.The composite anode being configured to by alloy particle powder is likely to because having larger surface area And strengthen feature unstable under high temperature.Therefore, although there is more substantial second element More conventional binary lithium alloy can be used as the anode of the embodiment according to present disclosure, But in some cases, ingot lithium alloy can be used for replacing above-mentioned binary lithium alloy with convenient Assemble and make and maintain higher heat stability and electrochemical function.These ingot lithiums close Gold can include Li-B-Mg or Li-Mg-xM, wherein M can represent silicon, aluminum, stannum, boron, Calcium, zinc or a combination thereof.
Means of differential scanning calorimetry (DSC) is used to assess different binary and ingot relative to pure lithium Lithium alloy, including Li-Mg, Li-B-Mg, Li-B, Li-Si and Li-Al.Fig. 4 describes In lithium metal pure within the temperature range of room temperature to about 260 DEG C, Li-B-Mg (correspondence Percentage by weight is 64:32:4), Li-Si (corresponding percentage by weight be 44:56) and The hot-fluid (W/g) of Li-Al (corresponding percentage by weight the is 27:73) DSC to temperature The result analyzed.When being estimated in this temperature range, pure lithium is at about 180 DEG C Endothermic peak expected from lower display.Find that Li-Al and Li-Si be not in this temperature range Maximum under melt.Li-B-Mg and Li-B also about 180 DEG C to 190 DEG C at aobvious Show endothermic peak, show the pure lithium metal corresponding to being limited in more high-melting-point alloy matrix The suppressed thermal behavior of fusing.
Return to be incorporated to the device formed as the embodiment according to present disclosure The electrolyte of a part, organic bath has been used in some commercial battery, but its quilt Confirm the electrochemical appliance not being suitable under extreme conditions running.Therefore, according to this The device that the embodiment of disclosure is formed may be incorporated into non-volatile ionic liquid electrolytic Matter is to be significantly expanded the temperature range of the device in high temperature is applied.Ionic liquid is electrolysed Matter chemically stable and generally in temperature range of operation with cathode material and anode material Both are compatible.In addition it is the most thermally-stabilised, and it is generally of low-down Vapour pressure.Additionally, be incorporated to the device of ionic liquid electrolyte generally at temperature range of operation The specific ionic conductivity of interior maintenance.
Lithium salts, as Li-TFSI may be dissolved in the one of several ionic liquids, wherein salt There is the concentration of 0.1M to 1.0M, to form the embodiment according to present disclosure Ionic liquid electrolyte.The ionic liquid that can use according to the embodiment of present disclosure The embodiment of body is including but not limited to EMI [1-ethyl-3-methylimidazole quinoline double (three Fluorine methylsulfonyl) imines], MPP [1-methyl isophthalic acid propylpiperdine double (fluoroform sulphonyl) Acid imide], BMP [1-butyl-1-crassitude double (fluoroform sulphonyl) acid imide], BTMA [double (fluoroform sulphonyl) imines of butyl trimethyl ammonium], DEMMoEA [diethyl Double (fluoroform sulphonyl) imines of methyl-(methoxyethyl) ammonium], have similarity other from Sub-liquid and a combination thereof.
Use thermogravimetric analysis (TGA) by scanning from room temperature percentage ratio for weight loss Every kind of above-mentioned ionic liquid electrolyte is assessed to the temperature of about 260 DEG C.Fig. 5 describes For by molten in including EMI, MPP, BMP and the EMI mixed with DEC Solve lithium salts and the different ionic liquid electrolyte that formed from room temperature to about 400 DEG C TGA data.Find that different electrolyte is thermally-stabilised in the case of weight loss reduction arrives About 350 DEG C.The EMI mixed with about 20% weight ratio DEC is being heated approximately to Causing organic bath to evaporate when 100 DEG C, residue EMI maintains it across test run simultaneously The stability of temperature range.
Come (straight from room temperature in temperature range additionally, perform means of differential scanning calorimetry (DSC) To about 260 DEG C) in the different ionic liquid electrolyte of assessment.Return to Fig. 6, Fig. 6 Describe for the ionic liquid formed by dissolving lithium salts in EMI, MPP and BMP The hot-fluid (W/g) of the body electrolyte dsc analysis result to temperature；But in target temperature Significant reaction is not found in the range of degree.It practice, the DSC data table described in Fig. 6 The bright decomposition being substantially absent to these ionic liquid electrolytes or chemical reaction are relevant Thermal change.
Additionally, test different in the presence of selected negative electrode and anode assemblies Ionic liquid electrolyte.These test requests are by a small pieces of solid anode material or negative electrode material Material is placed individually in electrolyte solution.Individual other negative electrode/electrolyte and anode/electrolyte are mixed Compound is then subjected to DSC and experimentally scans.Fig. 7 and Fig. 8 describes different ionic liquid The CF of electrolytexNegative electrode/electrolyte and the DSC of lithio anode/electrolyte half cell configuration Analyze.Find different ionic liquid electrolytes and selected negative electrode and anode material tool There is the good compatibility.For example, it was discovered that different anode materials is not electrolysed at ionic liquid Too much reactivity is shown in the presence of matter.
In another embodiment of present disclosure, including ionic liquid and Organic Electricity The hydridization electrolyte of the mixture solving matter can be used for expanding further temperature range of operation.This The ionic liquid ratio of sample a kind of hydridization electrolyte can include the institute of about 50% to 99% Obtain compositions.
Return to be incorporated to the device formed as the embodiment according to present disclosure The crust of the device of a part, described crust of the device can be made up of one or more materials, bag Include but be not necessarily limited to rustless steel, high nickel and stainless steel, titanium, nonmetal-coated rustless steel, Precious metal electroplating rustless steel or for other assembly of device the most inert other Material.Such a shell can provide capsul across temperature range of operation for device.
Apparatus structure can include the one of multiple structure, ties including but not limited to bobbin Structure, thin layer coating, spiral winding structure and/or medium bed package structure.Spiral winding Structure provides bigger metal exposed area and bigger anode/cathode interfacial area, leads Cause higher self discharge possible in high temperature electrochemical device.Spiral winding structure and bobbin Structure is compared and be may also include more inertia assembly, and it may cause the relatively mental retardation of device Metric density.
Barrier film can be used in the embodiment of present disclosure with by the set of cells in device Part (anode, negative electrode and electrolyte) is separately.Barrier film is generally at temperature range of operation interior-heat Stable and with other assembly chemical compatibility.Additionally, barrier film should have good dielectricity Can, there is higher electric insulation and permeability for liquids and ion transmission.According to the disclosure The barrier film of the embodiment of content can including but not limited to fibrous glass, PTFE, Polyimides and porous ceramics, such as aluminium oxide, silicon dioxide or zirconium oxide.Two barrier films Combination can also be incorporated to according in the device of the embodiment of present disclosure.As one Individual embodiment, compatible with lithium or lithium alloy and therefore PTFE can use the second barrier film Use PTFE to come towards negative electrode towards anode simultaneously.
The embodiment of present disclosure relates to the battery that can at high temperature use.Such one Plant the CF that battery can include having the x value of about 0.9xNegative electrode and there is corresponding weight ratio The Li-B-Mg anode of 64:32:4.The double fluoroforms being dissolved in MPP by 0.5M The ionic liquid electrolyte that sulfimide lithium (LiTFSI) forms can be used for present disclosure This embodiment in.Battery may also include by having about 60% porosity and 39 The two layers of polyimide of μ m thick, fibrous glass, aluminium oxide, silicon dioxide, oxidation Zirconium or the barrier film of PTFE composition.Netted collector body and collector body and shell two can be used Person can include nickel, rustless steel, aluminum, titanium, silver, gold, carbon cloth or carbon cladding rustless steel or Titanium.As it is shown in figure 9, the battery formed according to this embodiment can end at 2.0V The lower offer operation time of about 300 to 400 hours, average cathode utilization rate is of about 89%.However, it should be understood that because of such as by high viscosity at room temperature and non-optimized electrode shape Become and cause and the factor of electrode wettability bad between ionic liquid electrolyte The operation time at room temperature may shorter (in the range of 5 to 15 hours), put Electricity speed is relatively low.
Figure 10 describes running at 225 DEG C according to the embodiment of present disclosure The voltage curve of high-temperature battery.This test in, battery before electric discharge in short-circuit conditions Under be exposed to and mutually synthermal reach about 350 hours.It is exposed under the blanking voltage of 2.5 volts Stop.This discharge curve shows good voltage behavior, without as lithium-thionyl chloride electricity The voltage delay effect being passivated or being correlated with of problem present in the chemistry of pond.
Battery or device that embodiment according to present disclosure is formed can be from subzero Degree Celsius to give from well bore face travel across well pit shaft oil/gas exploitation and produce work Run in the wide temperature range of some maximum temperatures needed for tool power supply.This device also may be used Be arranged on different depth that oil/gas well disposes and polygon on telemetry communication repeater Run in maximum temperature district.Use the device that the embodiment according to present disclosure is formed It is also possible to be suitable for use in well monitoring, drill and measure, detect and the length of other field use Phase installs.The offer of these devices is better than the battery with the formation of standard lithium-thionyl chloride chemistry Performance and without taking in terms of high volume density, wide running temperature or user interface friendliness House.
The electrochemical appliance that embodiment according to present disclosure is formed can be also used for Outside oilfield applications application, including but not limited to space flight, space probation, automobile Monitoring tire pressure, medical treatment and military defense application.Such as, according to present disclosure The high-temperature battery that embodiment is formed can be used for replacing and is usually used in showing of monitoring tire pressure There is LiMnO2Battery.
Although having described present disclosure in detail, it is to be appreciated that can be various to carrying out herein Change, substitute and be altered without departing from present disclosure as defined in appended claims Spirit and scope.Additionally, the scope of subject application is not intended to be limited in description Described technique, machine, manufacture, material composition, means, method and steps specific Embodiment.One of ordinary skill in the art is easily understood from present disclosure, can root Use execution essentially identical to corresponding embodiment as herein described according to present disclosure Function or realize the existing of the result essentially identical to corresponding embodiment as herein described Or technique, machine, manufacture, material composition, means, method or the step of exploitation in the future. Therefore, include in the range of appended claims are directed at it these techniques, machine, manufacture, Material composition, means, method or step.

Claims (20)

1. the method powered for downhole operations, comprises:
Being that downhole operations is powered with electrochemical appliance, described electrochemical appliance comprises:
Negative electrode；
Lithio anode；
Ionic liquid electrolyte, wherein said ionic liquid electrolyte is by ion Liquid dissolves lithium salts and is formed；With
Barrier film,
Wherein said electrochemical appliance is at least transported at a temperature of 180 DEG C to 200 DEG C OK.
Method the most according to claim 1, wherein said ionic liquid selects From: 1-methyl isophthalic acid propylpiperdine double (fluoroform sulphonyl) acid imide, 1-butyl Double (fluoroform sulphonyl) acid imide of-1-crassitude and mixture thereof.
Method the most according to claim 1, wherein said ionic liquid is electrolysed Matter is dissolved in double (fluoroform sulphonyl) acid imide of 1-methyl isophthalic acid propylpiperdine Double (fluoroform sulphonyl) imide lis that concentration is 0.1 to 1.0M.
Method the most according to claim 1, wherein said negative electrode is by having Chemical formula CFxPerfluorocarbon formed, wherein x is in the scope of 0.3 to 1.
Method the most according to claim 4, wherein said negative electrode is without table Formed in the case of the activating agent of face.
Method the most according to claim 1, wherein said electrochemical appliance is also Comprise by least one collector body formed of llowing group of materials: Stainless steel 316, silver, Gold, platinum, carbon cloth, carbon cladding titanium, precious metal electroplating rustless steel and carbon cladding are stainless Steel.
Method the most according to claim 1, wherein said negative electrode is forced into bubble To form collector body on foam or grid.
Method the most according to claim 1, wherein said electrochemical appliance is also Comprise:
By at least one shell formed of llowing group of materials: Stainless steel 316, nickel close Gold 625, carbon cladding titanium, precious metal electroplating rustless steel and nonmetal-coated rustless steel.
Method the most according to claim 7, wherein said negative electrode is directly attached To described shell.
Method the most according to claim 1, wherein said lithio anode selects From:
There is chemical formula LixMyBianry alloy, there is chemical formula Li1-xMxTwo Unit's alloy and the ingot alloy of Li-B-Mg, wherein M is boron.
11. methods according to claim 1, wherein said lithio anode is There is the ingot alloy that respective weight ratio is about the Li-B-Mg of 64:32:4.
12. methods according to claim 1, wherein said electrochemical appliance Have selected from the structure of group including having structure:
Bobbin structure, thin layer coating, spiral winding structure and medium bed package structure.
13. methods according to claim 1, wherein said barrier film is polyamides Imines barrier film.
14. methods according to claim 1, wherein said downhole operations is Selected from including at least one of following group:
Oil/gas exploitation, oil/gas production, telemetry communication repeater, well monitoring/measure, And drilling operation.
15. methods according to claim 1, wherein said electrochemical appliance At least run at a temperature of 180 DEG C to 240 DEG C.
16. methods according to claim 1, wherein said electrochemical appliance At least run at a temperature of 180 DEG C to 260 DEG C.
17. methods powered for downhole operations, comprise:
Being that downhole operations is powered with battery, described battery comprises:
There is chemical formula CFxPerfluorocarbon negative electrode, wherein x 0.3 to 1 model In enclosing；
Li-B-Mg alloy or Li-B alloy anode；
Ionic liquid electrolyte, wherein said ionic liquid electrolyte is by ion Dissolving lithium salts in liquid and formed, described ionic liquid is selected from: 1-methyl isophthalic acid propyl group Double (fluoroform sulphonyl) acid imide of piperidines, 1-butyl-1-crassitude are double (fluoroform sulphonyl) acid imide and mixture thereof；With
Polyimide diaphragm,
Wherein said battery at least runs at a temperature of 180 DEG C to 220 DEG C.
18. methods according to claim 17, wherein said ionic liquid electricity Solve matter and be dissolved in double (fluoroform sulphonyl) acid imide of 1-methyl isophthalic acid propylpiperdine In double (fluoroform sulphonyl) imide lis that concentration is 0.1 to 1.0M.
19. methods according to claim 17, wherein said battery also comprises By at least one collector body formed of llowing group of materials: Stainless steel 316, silver, gold, Platinum, carbon cloth, carbon cladding titanium, precious metal electroplating rustless steel and carbon cladding rustless steel.
20. methods according to claim 17, wherein said battery also wraps Contain:
By at least one shell formed of llowing group of materials: Stainless steel 316, nickel close Gold 625, carbon cladding titanium, precious metal electroplating rustless steel and nonmetal-coated rustless steel.
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